Sedlak Jane A, Vishnoi Manal, Forsch Kiefer, Bhadha Pazinah, Aarons Sarah M, Grassian Vicki H
Department of Chemistry and Biochemistry, University of California San Diego, 9500 Gilman Drive, La Jolla, California 92093, United States.
Geoscience Research Division, Scripps Institution of Oceanography, University of California San Diego, 9500 Gilman Dr #0220, La Jolla, California 92093, United States.
ACS Earth Space Chem. 2024 Nov 13;8(12):2463-2473. doi: 10.1021/acsearthspacechem.4c00212. eCollection 2024 Dec 19.
As wildfire events become more frequent, there is a need to better understand the impact of smoke on the environment and human health. Smoke, or biomass burning aerosol (BBA), can undergo atmospheric processing changing its chemical and optical properties. We examined the interactions between four lignin pyrolysis products (catechol, syringol, syringic acid, and vanillic acid) and three BBA-relevant iron oxide mineral phases (hematite, maghemite, and magnetite) using attenuated total reflectance-Fourier transform infrared spectroscopy and dissolved iron measurements to better understand how atmospheric processing changes concentrations of soluble iron, iron oxidation state, and brown carbon abundance. Reductive dissolution was the primary dissolution mechanism for catechol and syringol, which led to a substantial amount of iron release ( < 0.05), whereas syringic and vanillic acids had little impact on dissolution. Comparisons with other BBA relevant compounds highlight the importance of both steric and electronic structures in the reductive dissolution process. The maghemite and magnetite phases, which are more likely to be present in BBA, released significantly more dissolved iron than hematite ( < 0.05), emphasizing the need to use BBA relevant iron oxide proxies in laboratory studies. This work provides insight into observations of iron dissolution and transformation of organics in BBA.
随着野火事件变得越来越频繁,有必要更好地了解烟雾对环境和人类健康的影响。烟雾,即生物质燃烧气溶胶(BBA),会经历大气过程,改变其化学和光学性质。我们使用衰减全反射傅里叶变换红外光谱和溶解铁测量方法,研究了四种木质素热解产物(儿茶酚、丁香酚、丁香酸和香草酸)与三种与BBA相关的氧化铁矿物相(赤铁矿、磁赤铁矿和磁铁矿)之间的相互作用,以更好地了解大气过程如何改变可溶性铁的浓度、铁的氧化态和棕碳丰度。还原溶解是儿茶酚和丁香酚的主要溶解机制,这导致大量铁释放(<0.05),而丁香酸和香草酸对溶解影响很小。与其他与BBA相关的化合物的比较突出了空间结构和电子结构在还原溶解过程中的重要性。更有可能存在于BBA中的磁赤铁矿和磁铁矿相释放的溶解铁比赤铁矿显著更多(<0.05),强调了在实验室研究中使用与BBA相关的氧化铁替代物的必要性。这项工作为BBA中铁溶解和有机物转化的观测提供了见解。